大气中草酸根水合物光电子能谱与红外谱理论研究

J4 ›› 2016, Vol. 33 ›› Issue (5): 524-529.

大气中草酸根水合物光电子能谱与红外谱理论研究

刘议蓉¹,黄腾¹,姜帅¹,张杨¹,彭秀球¹,黄伟¹,张为俊²

中国科学院安徽光学精密机械研究所大气物理化学研究室，安徽合肥 230031

收稿日期:2015-04-29 修回日期:2015-06-30 出版日期:2016-09-28 发布日期:2016-09-28

Theoretical investigation of photoelectron and infrared spectroscopy of hydrated oxalate in atmosphere

Liu Yi-Rong, Huang Teng, Jiang Shuai, Zhang Yang, Peng Xiu-Qiu, Huang Wei*, Zhang Wei-Jun

Laboratory of Atmospheric Physico-Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China

Received:2015-04-29 Revised:2015-06-30 Published:2016-09-28 Online:2016-09-28

摘要/Abstract

摘要： 离子诱导成核是大气中重要的成核类型，也是大气中新粒子的主要来源之一，它能对大气中新粒子的形成产生重要的影响。通过草酸根水合物的光电子能谱和红外谱模拟发现水分子的个数会影响团簇的稳定性。相对于C2O 42?(H2O)3 团簇分子第四个水分子的加入，能够有效地稳定草酸根分子上两个发生库伦排斥的电子。草酸根水合物团簇中水分子之间的相互作用要弱于水与草酸根之间的相互作用。红外谱的模拟展示水分子的个数对草酸根的核结构影响较小。

关键词: 光谱学，红外谱，团簇，氢键

Abstract: Ion-induced nucleation is a very important nucleation type, and it is also one of the main sources of new particles in the atmosphere. It has a significant impact to the formation of new particles in the atmosphere. By the simulation of photoelectron and infrared spectroscopy of hydrated oxalate, we found the number of water can affect the stability of cluster molecule. With respect to C2O 42?(H2O)3 cluster molecule, the fourth water molecule can effectively stabilize electrons with coulomb repulsion on the oxalate molecule. The interaction between water molecules is weak than the interaction between water and oxalate molecule in the hydrated. The simulated infrared spectroscopy shows the number of water molecules have a little effect for the nuclear structure of oxalate.

Key words: Spectroscopy; Infrared spectroscopy; Cluster; Hydrogen bond

刘议蓉黄腾姜帅张杨彭秀球黄伟张为俊. 大气中草酸根水合物光电子能谱与红外谱理论研究[J]. J4, 2016, 33(5): 524-529.

Liu Yi-Rong, Huang Teng, Jiang Shuai, Zhang Yang, Peng Xiu-Qiu, Huang Wei*, Zhang Wei-Jun. Theoretical investigation of photoelectron and infrared spectroscopy of hydrated oxalate in atmosphere[J]. J4, 2016, 33(5): 524-529.

参考文献

[1] U. Lohmann, and J. Feichter. Global indirect aerosol effects: a review [J]. Atmos. Chem. Phys., 2005, 5: 715-737.
[2] A. Nel. Air pollution-related illness: Effects of particles [J]. Science, 2005, 308: 804-806.
[3] C. A. Pope, R. T. Burnett, M. J. Thun, E. E. Calle, D. Krewski, K. Ito, and G. D. Thurston. Lung cancer, cardiopulmonary mortality, and long-term exposure to fine particulate air pollution [J]. Jama-j. Am. Med. Assoc., 2002, 287: 1132-1141.
[4] R. Bascom, P. A. Bromberg, D. A. Costa, R. Devlin, D. W. Dockery, M. W. Frampton, W. Lambert, J. M. Samet, F. E. Speizer, and M. Utell. Health effects of outdoor air pollution [J]. Am. J. Resp. Crit. Care, 1996, 153: 3-50.
[5] A. Ibald-Mulli, H. E. Wichmann, W. Kreyling, and A. Peters. Epidemiological evidence on health effects of ultrafine particles [J]. J. Aerosol. Med., 2002, 15: 189-201.
[6] C. A. Brock, P. Hamill, J. C. Wilson, H. H. Jonsson, and K. R. Chan. PARTICLE FORMATION IN THE UPPER TROPICAL TROPOSPHERE - A SOURCE OF NUCLEI FOR THE STRATOSPHERIC AEROSOL [J]. Science, 1995, 270: 1650-1653.
[7] M. de Reus, J. Strom, J. Curtius, L. Pirjola, E. Vignati, F. Arnold, H. C. Hansson, M. Kulmala, J. Lelieveld, and F. Raes. Aerosol production and growth in the upper free troposphere [J]. J. Geophys. Res.-Atmospheres, 2000, 105: 24751-24762.
[8] R. J. Weber, P. H. McMurry, R. L. Mauldin, D. J. Tanner, F. L. Eisele, A. D. Clarke, and V. N. Kapustin. New particle formation in the remote troposphere: A comparison of observations at various sites [J]. Geophys. Res. Lett., 1999, 26: 307-310.
[9] A. D. Clarke, F. Eisele, V. N. Kapustin, K. Moore, D. Tanner, L. Mauldin, M. Litchy, B. Lienert, M. A. Carroll, and G. Albercook. Nucleation in the equatorial free troposphere: Favorable environments during PEM-Tropics [J]. J. Geophys. Res.-Atmospheres, 1999, 104: 5735-5744.
[10] J. M. Makela, P. Aalto, V. Jokinen, T. Pohja, A. Nissinen, S. Palmroth, T. Markkanen, K. Seitsonen, H. Lihavainen, and M. Kulmala. Observations of ultrafine aerosol particle formation and growth in boreal forest [J]. Geophys. Res. Lett., 1997, 24: 1219-1222.
[11] I. G. Kavouras, N. Mihalopoulos, and E. G. Stephanou. Formation and gas/particle partitioning of monoterpenes photo-oxidation products over forests [J]. Geophys. Res. Lett., 1999, 26: 55-58.
[12] W. R. Leaitch, J. W. Bottenheim, T. A. Biesenthal, S. M. Li, P. S. K. Liu, K. Asalian, H. Dryfhout-Clark, F. Hopper, and F. Brechtel. A case study of gas-to-particle conversion in an eastern Canadian forest [J]. J. Geophys. Res.-Atmospheres, 1999, 104: 8095-8111.
[13] C. O'Dowd, G. McFiggans, D. J. Creasey, L. Pirjola, C. Hoell, M. H. Smith, B. J. Allan, J. M. C. Plane, D. E. Heard, J. D. Lee, M. J. Pilling, and M. Kulmala. On the photochemical production of new particles in the coastal boundary layer [J]. Geophys. Res. Lett., 1999, 26: 1707-1710.
[14] R. J. Weber, P. H. McMurry, L. Mauldin, D. J. Tanner, F. L. Eisele, F. J. Brechtel, S. M. Kreidenweis, G. L. Kok, R. D. Schillawski, and D. Baumgardner. A study of new particle formation and growth involving biogenic and trace gas species measured during ACE 1 [J]. J. Geophys. Res.-Atmospheres, 1998, 103: 16385-16396.
[15] C. O. Stanier, A. Y. Khlystov, and S. N. Pandis. Nucleation events during the Pittsburgh air quality study: Description and relation to key meteorological, gas phase, and aerosol parameters [J]. Aerosol. Sci. Tech., 2004, 38: 253-264.
[16] C. A. Brock, F. Schroder, B. Karcher, A. Petzold, R. Busen, and M. Fiebig. Ultrafine particle size distributions measured in aircraft exhaust plumes [J]. J. Geophys. Res.-Atmospheres, 2000, 105: 26555-26567.
[17] Lin Xiao-xiao, Liu Yi-rong, Yan Li-li, et al. Advances in Atmospheric Criegee intermediates detection methods [J]. Chinese Journal of Quantum Electronics(量子电子学报), 2015, 32:129-136(in Chinese).
[18] K. J. Taylor, C. L. Pettiettehall, O. Cheshnovsky, and R. E. Smalley. ULTRAVIOLET PHOTOELECTRON-SPECTRA OF COINAGE METAL-CLUSTERS [J]. J. Chem. Phys., 1992, 96: 3319-3329.
[19] F. Yu, and R. P. Turco. Ultrafine aerosol formation via ion‐mediated nucleation [J]. Geophys. Res. Lett., 2000, 27: 883-886.
[20] X. B. Wang, X. Yang, J. B. Nicholas, and L. S. Wang. Photodetachment of hydrated oxalate dianions in the gas phase, C2O42-(H2O)n (n=3-40): From solvated clusters to nanodroplet [J]. J. Chem. Phys., 2003, 119: 3631-3640.
[21] V. M. Rosas-García, I. del Carmen Sáenz-Tavera, V. J. Rodríguez-Herrera, and B. R. Garza-Campos. Microsolvation and hydration enthalpies of CaC2O4 (H2O)n (n= 0-16) and C2O42-(H2O)n (n= 0-14): an ab initio study [J]. J. Mol. Model., 2013, 19: 1459-1471.
[22] B. Gao, and Z.-f. Liu. First Principles Study on the Solvation and Structure of C2O42-(H2O)n, n= 6-12 [J]. J. Phys. Chem. A, 2005, 109: 9104-9111.
[23] K. H. Weber, F. J. Morales, and F.-M. Tao. Theoretical Study on the Structure and Stabilities of Molecular Clusters of Oxalic Acid with Water [J]. J. Phys. Chem. A, 2012, 116: 11601-11617.
[24] D. J. Wales, and J. P. Doye. Global optimization by basin-hopping and the lowest energy structures of Lennard-Jones clusters containing up to 110 atoms [J]. J. Phys. Chem. A, 1997, 101: 5111-5116.
[25] Z. Li, and H. A. Scheraga. Monte Carlo-minimization approach to the multiple-minima problem in protein folding [J]. Proc. Natl. Acad. Sci. U. S. A., 1987, 84: 6611-6615.
[26] B. Delley. AN ALL-ELECTRON NUMERICAL-METHOD FOR SOLVING THE LOCAL DENSITY FUNCTIONAL FOR POLYATOMIC-MOLECULES [J]. J. Chem. Phys., 1990, 92: 508-517.